Crystalline thin films of cuprous selenide (Cu2Se) were electrodeposited at room temperature from an aqueous solution containing elemental precursors for Cu and Se, using a potential pulse version of atomic layer deposition. Cyclic voltammetry was used to estimate Anodic and Cathodic cycle potentials for the formation of Cu2Se, which were then examined to systematically optimize the cycle. Electron probe microanalysis was used to follow the Cu/Se atomic ratios as a function of the cycle parameters, and X-ray diffraction was used to investigate deposit structure: polycrystalline orthorhombic Cu2Se, with some cubic. Film thicknesses, from spectroscopic ellipsometry, were shown to be proportional to the number of cycles performed (0.02 nm/cycle), and scanning electron microscopy suggested that the deposits were consistent with layer-by-layer growth as a function of the number of cycles.